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NTA-Fe@PDA/H2O2 oxidation for removal of oxytetracycline hydrochloride from wastewater |
LIN Jia-wei1,2, SU Bing-qin1,2, LI Xing-fa1, WEI Yue-xing1, ZHENG Xiao-xiao1, ZHANG Xia-ling1, SONG Xin-tong1, ZHAO Wen-bo1,2 |
1. College of Environmental Science and Engineering, Taiyuan University of Technology, Jinzhong 030600, China; 2. Shanxi Municipal Engineering Graduate Education Innovation Center, Jinzhong 030600, China |
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Abstract In this paper, polydopamine (PDA) grafted with nitrilotriacetic acid(NTA)and Fe3+ were chelated to form Fenton catalyst. Advanced oxidation process of NTA-Fe@PDA activated H2O2 was used to remove oxytetracyclin hydrochloride (OTC) from wastewater. The material characterization analysis showed that NTA-Fe@PDA was a typical mesoporous structure, Fe successfully chelated with organic ligand, and the polymerization effect of PDA was good. The effects of H2O2 dosage, NTA-Fe@PDA dosage and initial pH value on the degradation of OTC were investigated. Experimental results indicated that the degradation rate of 20mg/L OTC reached 96.23% after reaction for 60min, under the conditions of 5mmol/L H2O2, 200mg/L NTA-Fe@PDA and initial pH 4.85. Free radical quenching experiments confirmed that ·OH was the main free radical for OTC degradation. The possible degradation path of OTC was inferred by LC-MS analysis. The degradation rate of OTC was still above 86.80% after NTA-Fe@PDA was reused for 8times. Fenton oxidation process of NTA-Fe@PDA provided a new idea and technical reference for the treatment of antibiotic wastewater.
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Received: 13 October 2023
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[1] Fischbach M A, Walsh C T. Antibiotics for emerging pathogens[J]. Science, 2009,325(5944):1089-1093. [2] Phillips I, Casewell M, Cox T, et al. Does the use of antibiotics in food animals pose a risk to human health?A critical review of published data[J]. The Journal of Antimicrobial Chemotherapy, 2004,53(1):28-52. [3] 尉小琴,仲世江.养殖业中抗生素的使用问题[J].畜牧兽医杂志, 2011,30(2):117-118. Wei X Q, Zhong S J. The use of antibiotics in aquaculture[J]. Journal of Animal Husbandry and Veterinary Medicine, 2011,30(2):117-118. [4] 杨硕.畜禽养殖废水的抗生素污染现状及检测方法[J].农业与技术, 2020,40(21):107-108. Yang S. Status and detection methods of antibiotic contamination in livestock and poultry wastewater[J]. Agriculture and Technology, 2020,40(21):107-108. [5] Ngigi A N, Ok Y S, Thiele-Bruhn S. Biochar-mediated sorption of antibiotics in pig manure[J]. Journal of Hazardous Materials, 2019, 364:663-670. [6] Wang D, Jia F, Wang H, et al. Simultaneously efficient adsorption and photocatalytic degradation of tetracycline by Fe-based MOFs[J]. Journal of Colloid and Interface Science, 2018,519:273-284. [7] Yi Q Z, Zhang Y, Gao Y X, et al. Anaerobic treatment of antibiotic production wastewater pretreated with enhanced hydrolysis:Simultaneous reduction of COD and ARGs[J]. Water Research, 2017, 110:211-217. [8] Liu M M, Ding R, Zhang Y, et al. Abundance and distribution of Macrolide-Lincosamide-Streptogramin resistance genes in an anaerobic-aerobic system treating spiramycin production wastewater[J]. Water Research, 2014,63:33-41. [9] He Y P, Tian Z, Yi Q Z, et al. Impact of oxytetracycline on anaerobic wastewater treatment and mitigation using enhanced hydrolysis pretreatment[J]. Water Research, 2020,187. [10] 宋成智,张娇,李依,等.Fenton和类Fenton技术处理水中盐酸四环素试验研究[J].工业用水与废水, 2021,52(1):16-21,35. Song C Z, Zhang J, Li Y, et al. Comparison of fenton and fenton-like technology for treatment of tetracycline hydrochloride in water[J]. Industrial Water&Wastewater, 2021,52(1):16-21,35. [11] 白晓龙,储海蓉,李亚,等.Fenton氧化技术去除水中抗生素污染现状[J].工业安全与环保, 2020,46(10):73-76. Bai X L, Chu H R, Li Y, et al. Present situation of fenton oxidation technology to remove antibiotic pollution[J]. Industrial Safety and Environmental Protection, 2020,46(10):73-76. [12] Qin Y, Song F, Ai Z, et al. Protocatechuic acid promoted alachlor degradation in Fe (III)/H2O2 fenton system[J]. Environmental Science&Technology, 2015,49(13):7948-7956. [13] Kopf S H, Henny C, Newman D K. Ligand-Enhanced Abiotic Iron Oxidation and the Effects of Chemical versus Biological Iron Cycling in Anoxic Environments[J]. Environmental Science&Technology, 2013,47(6):2602-2611. [14] Gan G, Liu J, Zhu Z, et al. A novel magnetic nanoscaled Fe3O4/CeO2 composite prepared by oxidation-precipitation process and its application for degradation of orange G in aqueous solution as Fenton-like heterogeneous catalyst[J]. Chemosphere, 2017,168:254-263. [15] Zhu Y, Zhu R, Xi Y, et al. Strategies for enhancing the heterogeneous Fenton catalytic reactivity:A review[J]. Applied Catalysis B-Environmental, 2019,255. [16] 杜思南,罗阳,左芳,等.聚多巴胺包覆Fe3O4纳米粒子异相芬顿催化降解亚甲基蓝[J].精细化工, 2017,34(6):676-681. Du S N, Luo Y, Zuo F, et al. Polydopamine-coated Fe3O4 nanoparticles as heterogeneous fenton catalysts for degradation of Methylene Blue[J]. Fine Chemicals, 2017,34(6):676-681. [17] Zhou Z, Liu R. Fe3O4@polydopamine and derived Fe3O4@carbon core-shell nanoparticles:Comparison in adsorption for cationic and anionic dyes[J]. Colloids and Surfaces a-Physicochemical and Engineering Aspects, 2017,522:260-265. [18] 郁佳程,杨璐阳,王励珽,等.基于聚多巴胺的环境功能材料吸附水体重金属的研究进展[J].环境化学, 2021,40(7):2204-2216. Yu J C, Yang L Y, Wang L T, et al. Research progress of polydopamine-based environmental functional materials for the adsorption of the heavy metals in water[J]. Environmental Chemicals, 2021,40(7):2204-2216. [19] 陈贺,张帅其,赵致雪,等.多巴胺功能材料在水污染控制中的应用[J].化学进展, 2019,31(4):571-579. Cheng H, Zhang S Q, Zhao Z X, et al. Application of dopamine functional materials in water pollution control[J]. Progress In Chemistry, 2019,31(4):571-579. [20] Liu Y, Ai K, Lu L. Polydopamine and its derivative materials:synthesis and promising applications in energy, environmental, and Biomedical Fields[J]. Chemical Reviews, 2014,114(9):5057-5115. [21] Kumar T N, Sivabalan S, Chandrasekaran N, et al. Ferrocene-functionalized polydopamine as a novel redox matrix for H2O2 oxidation[J]. J Mater Chem B, 2014,2(36):6081-6088. [22] Zhang Y, Zhou M. A critical review of the application of chelating agents to enable Fenton and 1Fenton-like reactions at high pH values[J]. Journal of Hazardous Materials, 2019,362:436-450. [23] De Luca A, Dantas R F, Esplugas S. Study of Fe (III)-NTA chelates stability for applicability in photo-fenton at neutral pH[J]. Applied Catalysis B-Environmental, 2015,179:372-379. [24] De Laat J, Dao Y H, El Najjar N H, et al. Effect of some parameters on the rate of the catalysed decomposition of hydrogen peroxide by iron (III)-nitrilotriacetate in water[J]. Water Research, 2011,45(17):5654-5664. [25] Tachiev G I. Oxidation kinetics of organics using hydrogen peroxide catalyzed by "free" and complexed iron[M]. 1998. [26] Piccirillo G, Moreira-Santos M, Valega M, et al. Supported metalloporphyrins as reusable catalysts for the degradation of antibiotics:Synthesis, characterization, activity and ecotoxicity studies[J]. Applied Catalysis B-Environmental, 2021,282. [27] 姜成春,庞素艳,马军,等.钛盐光度法测定Fenton氧化中的过氧化氢[J].中国给水排水, 2006,(4):88-91. Jiang C C, Pang S Y, Ma J, et al. Determination of hydrogen peroxide in Fenton oxidation by titanium salt spectrophotometry[J]. China Water&Wastewater, 2006,(4):88-91. [28] 黄净,杨毅华,冯娟,等.环肽中酰胺键cis-/trans-异构化的相关研究进展[J].有机化学, 2020,40(6):1473-1483. Huang J, Yang Y H, Fen J, et al. Research progress on cis-/trans-isomerization of cyclic peptide[J]. Chinese Journal of Organic Chemistry, 2020,40(6):1473-1483. [29] Miao J, Geng W, Alvarez P J J, et al. 2D N-doped porous carbon derived from polydopamine-coated graphitic carbon nitride for efficient nonradical activation of peroxymonosulfate[J]. Environmental Science&Technology, 2020,54(13):8473-8481. [30] Wang H, Chen T, Chen D, et al. Sulfurized oolitic hematite as a heterogeneous Fenton-like catalyst for tetracycline antibiotic degradation[J]. Applied Catalysis B-Environmental, 2020,260. [31] Liang X, Yang S, Yang J, et al. Covalent immobilization of molecular complexes on metal-organic frameworks towards robust and highly efficient heterogeneous water oxidation catalysts[J]. Applied Catalysis B-Environmental, 2021,291. [32] Liu X F, Qin J A, Zhang X Y, et al. The mechanisms of HSA@PDA/Fe nanocomposites with enhanced nanozyme activity and their application in intracellular H2O2 detection[J]. Nanoscale, 2020,12(47):24206-24213. [33] Fan L, Xie J, Zhang Z, et al. Magnetically recoverable Fe3O4@polydopamine nanocomposite as an excellent co-catalyst for Fe3+reduction in advanced oxidation processes[J]. Journal of Environmental Sciences, 2020,92:69-78. [34] Kim Y, Huh S. Pore engineering of metal-organic frameworks:introduction of chemically accessible Lewis basic sites inside MOF channels[J]. Crystengcomm, 2016,18(20):3524-3550. [35] Mao Y, Wang P, Zhang D, et al. Accelerating Fe-III-aqua complex reduction in an efficient solid-liquid-interfacial fenton reaction over the Mn-CNH Co-catalyst at near-neutral pH[J]. Environmental Science&Technology, 2021,55(19):13326-13334. [36] Chen Y, Yang Z, Liu Y, et al. Fenton-like degradation of sulfamerazine at nearly neutral pH using Fe-Cu-CNTs and Al-0-CNTs for in-situ generation of H2O2/(OH)-O-center dot/O-2(center dot-)[J]. Chemical Engineering Journal, 2020,396. [37] 曾萍,刘诗月,张俊珂,等.芬顿法深度处理生物处理排水中的四环素抗性基因[J].中国环境科学, 2017,37(9):3315-3323. Zeng P, Liu S Y, Zhang J K, et al. advanced Fenton oxidation treatment of tetracycline resistance genes in effluent discharged from biological wastewater treatment[J]. China Environmental Science, 2017,37(9):3315-3323. [38] 杨远秀,姚创,刘晖,等.磁性Fen+@GO非均相Fenton催化氧化亚甲基蓝[J].中国环境科学, 2018,38(5):1719-1726. Yang Y X, Yao C, Liu H, et al. Heterogeneous fenton catalyzed oxidation of methylene blue by magnetic Fen+[J]. China Environmental Science, 2018,38(5):1719-1726. [39] Li M, He Z, Zhong H, et al.(Fe0.67Mn0.33) OOH riched in oxygen vacancies facilitated the PMS activation of modified EMR for refractory foaming agent removal from mineral processing wastewater[J]. Chemical Engineering Journal, 2022,441. [40] Xiao C, Hu Y, Li Q, et al. Degradation of sulfamethoxazole by super-hydrophilic MoS2sponge co-catalytic Fenton:Enhancing Fe2+/Fe3+cycle and mass transfer[J]. Journal of Hazardous Materials, 2023,458. [41] Mao X, Deng Z, Liu Y, et al. Iron single atoms and clusters anchored on natural N-doped nanocarbon with dual reaction sites as superior Fenton-like catalysts[J]. Applied Surface Science, 2022,597. [42] Li X, Huang X, Xi S, et al. Single cobalt atoms anchored on porous N-doped graphene with dual reaction sites for efficient fenton-like catalysis[J]. Journal of the American Chemical Society, 2018,140(39):12469-12475. [43] Wang W, Niu Q, Zeng G, et al. 1D porous tubular g-C3N4 capture black phosphorus quantum dots as 1D/0D metal-free photocatalysts for oxytetracycline hydrochloride degradation and hexavalent chromium reduction[J]. Applied Catalysis B-Environmental, 2020,273. [44] 谢金伶,蒲佳兴,李思域,等.钴锰硫化物活化过硫酸盐强化降解盐酸四环素[J].中国环境科学, 2023,43(2):544-551. Xie J L, Pu J X, Li S Y, et al. Enhanced degradation of tetracycline hydrochloride by cobalt-manganese sulfide activated peroxymonosulfate[J]. China Environmental Science, 2023,43(2):544-551. |
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